Revealing the Phonon Bottleneck Limit in Negatively Charged CdS Quantum Dots

Sherman, Skylar J.; Hou, Bokang; Coley-O’Rourke, Matthew J.; Shulenberger, Katherine E.; Pellows, Lauren M.; Rabani, Eran; Dukovic, Gordana

doi:10.1021/acsnano.4c15181

Revealing the Phonon Bottleneck Limit in Negatively Charged CdS Quantum Dots

Journal Article · Thu Feb 13 04:00:00 EST 2025 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.4c15181· OSTI ID:2565879

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Univ. of Colorado, Boulder, CO (United States)
University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
University of California, Berkeley, CA (United States)
Univ. of Colorado, Boulder, CO (United States); Brandeis Univ., Waltham, MA (United States)
University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Tel Aviv Univ. (Israel)

The capture of photoexcited hot electrons in semiconductors before they lose their excess energy to cooling is a long-standing goal in photon energy conversion. Semiconductor nanocrystals have large electron energy spacings that are expected to slow down electron relaxation by phonon emission, but hot electrons in photoexcited nanocrystals, nevertheless, cool rapidly by energy transfer to holes. This makes the intrinsic phonon-bottleneck-limited hot electron lifetime in nanocrystals elusive. For this work, we used a combination of theory and experiments to probe the hot-electron dynamics of negatively charged cadmium sulfide (CdS) colloidal quantum dots (QDs) in the absence of holes. Experiments found that these hot electrons cooled on a 100 ps time scale. Theoretical simulations predicted that pure phonon-bottleneck-limited hot electron cooling occurs on a similar time scale. This similarity suggests that the experimental measurements reflect the upper limit on the hot-electron lifetimes in these CdS QDs and the lower limit on the rates of processes that can harvest those hot electrons.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); USDOE Office of Science (SC), Advanced Scientific Computing Research (ASCR). Scientific Discovery through Advanced Computing (SciDAC)

Grant/Contract Number:: AC02-05CH11231; SC0022088

OSTI ID:: 2565879

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 7 Vol. 19; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Revealing the Phonon Bottleneck Limit in Negatively Charged CdS Quantum Dots

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